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DOE OSTI2021

Anthropogenic Perturbations to the Atmospheric Molybdenum Cycle

Abstract Molybdenum (Mo) is a key cofactor in enzymes used for nitrogen (N) fixation and nitrate reduction, and the low availability of Mo can constrain N inputs, affecting ecosystem productivity. Natural atmospheric Mo aerosolization and deposition from sources such as desert dust, sea‐salt spray, and volcanoes can affect ecosystem function across long timescales, but anthropogenic activities such as combustion, motor vehicles, and agricultural dust have accelerated the natural Mo cycle. Here we combined a synthesis of global atmospheric concentration observations and modeling to identify and estimate anthropogenic sources of atmospheric Mo. To project the impact of atmospheric Mo on terrestrial ecosystems, we synthesized soil Mo data and estimated the global distribution of soil Mo using two approaches to calculate turnover times. We estimated global emissions of atmospheric Mo in aerosols (<10 μm in diameter) to be 23 Gg Mo yr −1 , with 40%–75% from anthropogenic sources. We approximated that for the top meter of soil, Mo turnover times range between 1,000 and 1,000,000 years. In some industrialized regions, anthropogenic inputs have enhanced Mo deposition 100‐fold, lowering the soil Mo turnover time considerably. Our synthesis of global observational data, modeling, and a mass balance comparison with riverine Mo exports suggest that anthropogenic activity has greatly accelerated the Mo cycle, with potential to influence N‐limited ecosystems.

Wong, Michelle Y.↗

DOE OSTI2024

Constraining Present‐Day Anthropogenic Total Iron Emissions Using Model and Observations

Abstract Iron emissions from human activities, such as oil combustion and smelting, affect the Earth's climate and marine ecosystems. These emissions are difficult to quantify accurately due to a lack of observations, particularly in remote ocean regions. In this study, we used long‐term, near‐source observations in areas with a dominance of anthropogenic iron emissions in various parts of the world to better estimate the total amount of anthropogenic iron emissions. We also used a statistical source apportionment method to identify the anthropogenic components and their sub‐sources from bulk aerosol observations in the United States. We find that the estimates of anthropogenic iron emissions are within a factor of 3 in most regions compared to previous inventory estimates. Under‐ or overestimation varied by region and depended on the number of sites, interannual variability, and the statistical filter choice. Smelting‐related iron emissions are overestimated by a factor of 1.5 in East Asia compared to previous estimates. More long‐term iron observations and the consideration of the influence of dust and wildfires could help reduce the uncertainty in anthropogenic iron emissions estimates.

Meteorology & Atmospheric Sciences↗

DOE OSTI2021

Anthropogenic influence on extreme precipitation over global land areas seen in multiple observational datasets

The intensification of extreme precipitation under anthropogenic forcing is robustly projected by global climate models, but highly challenging to detect in the observational record. Large internal variability distorts this anthropogenic signal. Models produce diverse magnitudes of precipitation response to anthropogenic forcing, largely due to differing schemes for parameterizing subgrid-scale processes. Meanwhile, multiple global observational datasets of daily precipitation exist, developed using varying techniques and inhomogeneously sampled data in space and time. Previous attempts to detect human influence on extreme precipitation have not incorporated model uncertainty, and have been limited to specific regions and observational datasets. Using machine learning methods that can account for these uncertainties and capable of identifying the time evolution of the spatial patterns, we find a physically interpretable anthropogenic signal that is detectable in all global observational datasets. Machine learning efficiently generates multiple lines of evidence supporting detection of an anthropogenic signal in global extreme precipitation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Global net climate effects of anthropogenic reactive nitrogen

Anthropogenic activities have substantially enhanced the loadings of reactive nitrogen (Nr) in the Earth system since pre-industrial times, contributing to widespread eutrophication and air pollution. Increased Nr can also influence global climate through a variety of effects on atmospheric and land processes but the cumulative net climate effect is yet to be unravelled. Here we show that anthropogenic Nr causes a net negative direct radiative forcing of –0.34 [–0.20, –0.50] W m –2 in the year 2019 relative to the year 1850. This net cooling effect is the result of increased aerosol loading, reduced methane lifetime and increased terrestrial carbon sequestration associated with increases in anthropogenic Nr, which are not offset by the warming effects of enhanced atmospheric nitrous oxide and ozone. Future predictions using three representative scenarios show that this cooling effect may be weakened primarily as a result of reduced aerosol loading and increased lifetime of methane, whereas in particular N 2 O-induced warming will probably continue to increase under all scenarios. Our results indicate that future reductions in anthropogenic Nr to achieve environmental protection goals need to be accompanied by enhanced efforts to reduce anthropogenic greenhouse gas emissions to achieve climate change mitigation in line with the Paris Agreement.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Nature-based solutions in mountain catchments reduce impact of anthropogenic climate change on drought streamflow

Quantifying how well Nature-based Solutions can offset anthropogenic climate change impacts is important for adaptation planning, but has rarely been done. Here we show that a widely-applied Nature-based Solution in South Africa – invasive alien tree clearing – reduces the impact of anthropogenic climate change on drought streamflow. Using a multi-model joint-attribution of climate and landscape-vegetation states during the 2015–2017 Cape Town “Day Zero” drought, we find that anthropogenic climate change reduced streamflow by 12–29% relative to a counterfactual world with anthropogenic emissions removed. This impact on streamflow was larger than corresponding reductions in rainfall (7–15%) and reference evapotranspiration (1.7–2%). Clearing invasive alien trees could have ameliorated streamflow reductions by 3–16% points for moderate invasions levels. Preventing further invasive alien tree spread avoided potential additional reductions of 10–27% points. Total clearing could not have offset the anthropogenic climate change impact completely. Invasive alien tree clearing is an important form of catchment restoration for managing changing hydroclimatic risk, but will need to be combined with other adaptation options as climate change accelerates.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Fallowed agricultural lands dominate anthropogenic dust sources in California

Air pollution remains a major problem in many parts of California, significantly impacting public health and regional climate. However, the contribution of anthropogenic dust from agricultural sources, among major pollutants in California’s semi-arid Central Valley, remains largely unclear. Here, we used the Cropland Data Layer from the U.S. Department of Agriculture to identify crop types and land use/cover and leveraged satellite-derived estimates of major dust events between 2008 and 2022 over California. We identified fallowed land—an unplanted agricultural land parcel—as a key anthropogenic dust source in California. Specifically, we find that the Central Valley accounts for about 77% of total fallowed land areas in California, where they are associated with about 88% of major anthropogenic dust events. We also find that the geographic coverage of these fallowed lands expanded between 2008 and 2022 with associated increasing anthropogenic dust activities. Additionally, these anthropogenic dust activities are sensitive to the drought severity over the fallowed lands, with potential cumulative effects on downstream dust burden during prolonged multi-year drought conditions. Overall, our results have important implications for public health, including increased risk for Valley fever and for regional climates, such as increases in extreme precipitation and snowmelt over the Sierra Nevada.

Climate sciences↗

DOE OSTI2020

Development of a mineralogy-based anthropogenic combustion-iron emission inventory

Atmospheric supply of iron can modulate ocean biogeochemistry, due to its key role in global nitrogen and carbon cycles. Using a detailed technology-based methodology we revise total and soluble anthropogenic iron emissions and resolve iron into its mineral components, which allows modeling mineral-specific atmospheric reactions. The inclusion of metal smelting as an iron source, increases fine iron aerosol emissions (smaller than 1 µm) compared with most previous inventories. Different assumptions about solubility lead to estimates of 40-450 Gg/year deposition of soluble anthropogenic iron. When combined with dust and wildfires, the global total anthropogenic soluble iron deposition is 1900-2300 Gg/yr, so assumptions in anthropogenic inventories can affect estimates of global soluble iron supply by about 30%. In regions where marine primary productivity is iron-limited, anthropogenic combustion-iron contributes up to half of the atmospheric soluble iron flux to North Pacific Ocean.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Effective radiative forcing of anthropogenic aerosols in E3SM version 1: historical changes, causality, decomposition, and parameterization sensitivities

Abstract. The effective radiative forcing of anthropogenic aerosols (ERFaer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERFaer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERFaer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERFaer magnitude does not increase after around 1970. The ERFaer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERFaer). As suggested by a previous study, the large ERFaer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERFaer. The ERFaer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERFaer, it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Atmospheric Radiative and Oceanic Biological Productivity Responses to Increasing Anthropogenic Combustion‐Iron Emission in the 1850–2010 Period

Abstract Anthropogenic emission is an important component of the present‐day iron cycle yet its long‐term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy‐based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m 2 . We estimate that the CO 2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO 2 forcing of −0.002 to −0.16 W/m 2 . While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m 2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high‐latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Anthropogenic climate change impacts exacerbate summer forest fires in California

Record-breaking summer forest fires have become a regular occurrence in California. Observations indicate a fivefold increase in summer burned area (BA) in forests in northern and central California during 1996 to 2021 relative to 1971 to 1995. While the higher temperature and increased dryness have been suggested to be the leading causes of increased BA, the extent to which BA changes are due to natural variability or anthropogenic climate change remains unresolved. Here, we develop a climate-driven model of summer BA evolution in California and combine it with natural-only and historical climate simulations to assess the importance of anthropogenic climate change on increased BA. Our results indicate that nearly all the observed increase in BA is due to anthropogenic climate change as historical model simulations accounting for anthropogenic forcing yield 172% (range 84 to 310%) more area burned than simulations with natural forcing only. We detect the signal of combined historical forcing on the observed BA emerging in 2001 with no detectable influence of the natural forcing alone. In addition, even when considering fuel limitations from fire-fuel feedbacks, a 3 to 52% increase in BA relative to the last decades is expected in the next decades (2031 to 2050), highlighting the need for proactive adaptations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Anthropogenically driven climate and landscape change effects on inland water carbon dynamics: What have we learned and where are we going?

Inland waters serve as important hydrological connections between the terrestrial landscape and oceans but are often overlooked in global carbon (C) budgets and Earth System Models. Terrestrially derived C entering inland waters from the watershed can be transported to oceans but over 83% is either buried in sediments or emitted to the atmosphere before reaching oceans. Anthropogenic pressures such as climate and landscape changes are altering the magnitude of these C fluxes in inland waters. Here, we synthesize the most recent estimates of C fluxes and the differential contributions across inland waterbody types (rivers, streams, lakes, reservoirs, and ponds), including recent measurements that incorporate improved sampling methods, small waterbodies, and dried areas. Across all inland waters, we report a global C emission estimate of 4.40 Pg C/year (95% confidence interval: 3.95–4.85 Pg C/year), representing a 13% increase from the most recent estimate. In this work, we also review the mechanisms by which the most globally widespread anthropogenically driven climate and landscape changes influence inland water C fluxes. The majority of these drivers are expected to influence terrestrial C inputs to inland waters due to alterations in terrestrial C quality and quantity, hydrological pathways, and biogeochemical processing. We recommend four research priorities for the future study of anthropogenic alterations to inland water C fluxes: (1) before-and-after measurements of C fluxes associated with climate change events and landscape changes, (2) better quantification of C input from land, (3) improved assessment of spatial coverage and contributions of small inland waterbodies to C fluxes, and (4) integration of dried and drawdown areas to global C flux estimates. Improved measurements of inland water C fluxes and quantification of uncertainty in these estimates will be vital to understanding both terrestrial C losses and the “moving target” of inland water C emissions in response to rapid and complex anthropogenic pressures.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Multi-scale quantification of anthropogenic, fire, and drought-associated forest disturbances across the continental U.S., 2000–2014

Our understanding of broad-scale forest disturbances under climatic extremes remains incomplete. Drought, as a typical extreme event, is a key driver of forest mortality but there have been no reports on continental-scale quantification of its impact on forest mortality or how it compares to other natural or anthropogenic drivers. Thus, our ability to understand and predict broad-scale carbon cycling in response to changing climate and extreme events is limited. In this study, we applied an attribution approach based on different sources of data to quantify the area and potential carbon loss/transfer in continental U.S. (CONUS) from four types of disturbance: (1) anthropogenic (especially timber harvest); (2) fire; (3) drought-associated; and (4) other from 2000 to 2014. Our results showed that anthropogenic disturbances, fire, drought-associated disturbances, and other disturbances accounted for 54.3, 10.7, 12.7, and 22.3% of total canopy area loss, respectively. Anthropogenic disturbance was the most important driver contributing to 58.1% potential carbon loss/transfer in CONUS for 2000–2014. The potential carbon loss/transfer from natural disturbances (fire, drought, and other) for the same study period accounted for approximately 41.9% of the total loss/transfer from all agents, suggesting that natural disturbances also played a very important role in forest carbon turnover. Potential carbon loss/transfer associated with drought accounted for approximately 11.6% of the total loss/transfer in CONUS, which was of similar magnitude to potential carbon loss/transfer from fire (~11.0%). The other natural disturbance accounted for 19.3% of potential carbon loss/transfer. Our results demonstrated the importance of the impacts of various disturbances on forest carbon stocks at the continental scale, and the drought-associated carbon loss/transfer data developed here could be used for evaluating the performance of predictive models of tree mortality under droughts.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

City-Scale Building Anthropogenic Heating during Heat Waves

More frequent and longer duration heat waves have been observed worldwide and are recognized as a serious threat to human health and the stability of electrical grids. Past studies have identified a positive feedback between heat waves and urban heat island effects. Anthropogenic heat emissions from buildings have a crucial impact on the urban environment, and hence it is critical to understand the interactive effects of urban microclimate and building heat emissions in terms of the urban energy balance. Here we developed a coupled-simulation approach to quantify these effects, mapping urban environmental data generated by the mesoscale Weather Research and Forecasting (WRF) coupled to Urban Canopy Model (UCM) to urban building energy models (UBEM). We conducted a case study in the city of Los Angeles, California, during a five-day heat wave event in September 2009. We analyzed the surge in city-scale building heat emission and energy use during the extreme heat event. We first simulated the urban microclimate at a high resolution (500 m by 500 m) using WRF-UCM. We then generated grid-level building heat emission profiles and aggregated them using prototype building energy models informed by spatially disaggregated urban land use and urban building density data. The spatial patterns of anthropogenic heat discharge from the building sector were analyzed, and the quantitative relationship with weather conditions and urban land-use dynamics were assessed at the grid level. The simulation results indicate that the dispersion of anthropogenic heat from urban buildings to the urban environment increases by up to 20% on average and varies significantly, both in time and space, during the heat wave event. The heat dispersion from the air-conditioning heat rejection contributes most (86.5%) of the total waste heat from the buildings to the urban environment. We also found that the waste heat discharge in inland, dense urban districts is more sensitive to extreme events than it is in coastal or suburban areas. The generated anthropogenic heat profiles can be used in urban microclimate models to provide a more accurate estimation of urban air temperature rises during heat waves.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

On the attribution of the impacts of extreme weather events to anthropogenic climate change

Investigations into the role of anthropogenic climate change in extreme weather events are now starting to extend into analysis of anthropogenic impacts on non-climate (e.g. socio-economic) systems. However, care needs to be taken when making this extension, because methodological choices regarding extreme weather attribution can become crucial when considering the events’ impacts. The fraction of attributable risk (FAR) method, useful in extreme weather attribution research, has a very specific interpretation concerning a class of events, and there is potential to misinterpret results from weather event analyses as being applicable to specific events and their impact outcomes. Using two case studies of meteorological extremes and their impacts, we argue that FAR is not generally appropriate when estimating the magnitude of the anthropogenic signal behind a specific impact. Attribution assessments on impacts should always be carried out in addition to assessment of the associated meteorological event, since it cannot be assumed that the anthropogenic signal behind the weather is equivalent to the signal behind the impact because of lags and nonlinearities in the processes through which the impact system reacts to weather. Whilst there are situations where employing FAR to understand the climate change signal behind a class of impacts is useful (e.g. ‘system breaking’ events), more useful results will generally be produced if attribution questions on specific impacts are reframed to focus on changes in the impact return value and magnitude across large samples of factual and counterfactual climate model and impact simulations. We advocate for constant interdisciplinary collaboration as essential for effective and robust impact attribution assessments.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Applying Machine Learning and Bayesian Inference to Identify and Locate Moving Anthropogenic Sources Using Distributed Acoustic Sensing Data

Distributed acoustic sensing (DAS) systems, which use existing telecommunication fibers, offer high‐resolution capabilities ideal for recording anthropogenic sources. However, the complexity of urban environments and the large amount of data recorded by DAS require automated methods to efficiently detect and categorize anthropogenic sources. Here, we evaluate how well three machine learning models (k‐nearest neighbor [k‐NN], convolutional neural networks, and recurrent‐convolutional neural networks) can identify various anthropogenic sources recorded by DAS. Our findings reveal that both k‐NN and neural network methods perform well in high signal‐to‐noise ratio (SNR) settings. However, their accuracy decreases at SNRs <4. We also use Kalman filtering, a form of Bayesian inference, on backprojected locations of these sources to recover locations that generally fall within standard smartphone Global Positioning System errors. By combining machine learning and Kalman filter results, we calculate a multidimensional model of moving anthropogenic sources. These results demonstrate the potential of DAS data in urban seismology for accurately identifying and locating such sources. Depending on the research objectives, these sources can be further studied or filtered out to improve the quality of seismic data for earthquake studies. Such methods provide a valuable tool for urban seismology and seismic hazard analysis.

Luckie, Thomas William [Sandia National Laboratori↗

DOE OSTI2023

Updating and Evaluating Anthropogenic Emissions for NOAA’s Global Ensemble Forecast Systems for Aerosols (GEFS-Aerosols): Application of an SO 2 Bias-Scaling Method

We updated the anthropogenic emissions inventory in NOAA’s operational Global Ensemble Forecast for Aerosols (GEFS-Aerosols) to improve the model’s prediction of aerosol optical depth (AOD). We used a methodology to quickly update the pivotal global anthropogenic sulfur dioxide (SO 2 ) emissions using a speciated AOD bias-scaling method. The AOD bias-scaling method is based on the latest model predictions compared to NASA’s Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA2). The model bias was subsequently applied to the CEDS 2019 SO 2 emissions for adjustment. The monthly mean GEFS-Aerosols AOD predictions were evaluated against a suite of satellite observations (e.g., MISR, VIIRS, and MODIS), ground-based AERONET observations, and the International Cooperative for Aerosol Prediction (ICAP) ensemble results. The results show that transitioning from CEDS 2014 to CEDS 2019 emissions data led to a significant improvement in the operational GEFS-Aerosols model performance, and applying the bias-scaled SO 2 emissions could further improve global AOD distributions. The biases of the simulated AODs against the observed AODs varied with observation type and seasons by a factor of 3~13 and 2~10, respectively. The global AOD distributions showed that the differences in the simulations against ICAP, MISR, VIIRS, and MODIS were the largest in March–May (MAM) and the smallest in December–February (DJF). When evaluating against the ground-truth AERONET data, the bias-scaling methods improved the global seasonal correlation (r), Index of Agreement (IOA), and mean biases, except for the MAM season, when the negative regional biases were exacerbated compared to the positive regional biases. The effect of bias-scaling had the most beneficial impact on model performance in the regions dominated by anthropogenic emissions, such as East Asia. However, it showed less improvement in other areas impacted by the greater relative transport of natural emissions sources, such as India. The accuracies of the reference observation or assimilation data for the adjusted inputs and the model physics for outputs, and the selection of regions with less seasonal emissions of natural aerosols determine the success of the bias-scaling methods. A companion study on emission scaling of anthropogenic absorbing aerosols needs further improved aerosol prediction.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Increased importance of aerosol–cloud interactions for surface PM 2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions

Surface fine particulate matter (PM 2.5 ) pollution can be enhanced by feedback processes induced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). Many previous studies have reported enhanced PM 2.5 concentrations induced by ARIs and ACIs for episodic events in China. However, few studies have examined the changes in the ARI- and ACI-induced PM 2.5 enhancements over a long period, though the anthropogenic emissions have changed substantially in the last decade. In this study, we quantify the ARI- and ACI-induced PM 2.5 changes for 2013–2021 under different meteorology and emission scenarios using the Weather Research and Forecasting model with Chemistry (WRF-Chem), and we investigate the driving factors behind the changes. Our results show that, in January 2013, when China suffered from the worst PM 2.5 pollution, the PM 2.5 enhancement induced by ARIs in eastern China (5.59 µg m −3 ) was larger than that induced by ACIs (3.96 µg m −3 ). However, the ACI-induced PM 2.5 enhancement showed a significantly smaller decrease ratio (51 %) than the ARI-induced enhancement (75 %) for 2013–2021, making ACIs more important for enhancing PM 2.5 concentrations in January 2021. Our analyses suggest that the anthropogenic emission reductions played a key role in this shift. Owing to only anthropogenic emission reductions, the ACI-induced PM 2.5 enhancement decreased by 43 % in January, which was lower than the decrease ratio of the ARI-induced enhancement (57 %). The relative change in ARI- and ACI-induced PM 2.5 enhancement in July was similar to the pattern observed in January, caused by anthropogenic emission reductions. The primary reason for this phenomenon is that the decrease in ambient PM 2.5 for 2013–2021 caused a disproportionately small decrease in the liquid water path (LWP) and an increase in the cloud effective radius (Re) under the condition of high PM 2.5 concentrations. Therefore, the surface solar radiation attenuation (and, hence, the boundary layer height reduction) caused by ACIs decreased slower than that caused by ARIs. Moreover, the lower decrease ratio of the ACI-induced PM 2.5 enhancement was dominated by the lower decrease ratio of ACI-induced secondary PM 2.5 component enhancement, which was additionally caused by the smaller decrease ratio of the air temperature reduction and the relative humidity (RH) increase. Our findings indicate that, with the decrease in ambient PM 2.5 , the ACI-induced PM 2.5 enhancement inevitably becomes more important. This needs to be considered in the formulation of control policies to meet the national PM 2.5 air quality standard.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

General circulation models simulate negative liquid water path–droplet number correlations, but anthropogenic aerosols still increase simulated liquid water path

General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree.

54 ENVIRONMENTAL SCIENCES↗